Raziq Fazal, Feng Chengyang, Hu Miao, Zuo Shouwei, Rahman Mohammad Ziaur, Yan Yayu, Li Qiao-Hong, Gascon Jorge, Zhang Huabin
KAUST Catalysis Center (KCC), Division of Physical Science and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, P. R. China.
J Am Chem Soc. 2024 Jul 31;146(30):21008-21016. doi: 10.1021/jacs.4c05873. Epub 2024 Jun 13.
Photothermal hydrogenation of carbon dioxide (CO) into value-added products is an ideal solution for addressing the energy crisis and mitigating CO emissions. However, achieving high product selectivity remains challenging due to the simultaneous occurrence of numerous competing intermediate reactions during CO hydrogenation. We present a novel approach featuring isolated single-atom nickel (Ni) anchored onto indium oxide (InO) nanocrystals, serving as an effective photothermal catalyst for CO hydrogenation into methane (CH) with a remarkable near-unity (∼99%) selectivity. Experiments and theoretical simulations have confirmed that isolated Ni sites on the InO surface can effectively stabilize the intermediate products of the CO hydrogenation reaction and reduce the transition state energy barrier, thereby changing the reaction path to achieve ultrahigh selective methanation. This study provides comprehensive insights into the design of single-atom catalysts for the highly selective photothermal catalytic hydrogenation of CO to methane.
将二氧化碳（CO₂）光热加氢转化为高附加值产品是解决能源危机和减少CO₂排放的理想解决方案。然而，由于CO₂加氢过程中同时发生众多相互竞争的中间反应，实现高产物选择性仍然具有挑战性。我们提出了一种新颖的方法，即孤立的单原子镍（Ni）锚定在氧化铟（In₂O₃）纳米晶体上，作为一种有效的光热催化剂，用于将CO₂加氢转化为甲烷（CH₄），其选择性接近完美（约99%）。实验和理论模拟证实，In₂O₃表面的孤立Ni位点可以有效地稳定CO₂加氢反应的中间产物，并降低过渡态能垒，从而改变反应路径以实现超高选择性甲烷化。这项研究为设计用于将CO₂高选择性光热催化加氢制甲烷的单原子催化剂提供了全面的见解。
